Response to Comment on “Following molecular mobility during chemical reactions: 
no evidence for active propulsion” and “Molecular diffusivity of click reaction 
components: the diffusion enhancement question”

Fillbrook, Lucy L.; Günther, Jan-Philipp; Majer, Günter; O’Leary, Daniel J.; Price, William S.; Ryswyk, Hal Van; Fischer, Peer; Beves, Jonathon E.

doi:10.1021/jacs.2c02830

Item

ITEM ACTIONSEXPORT

Add to Basket

Local TagsRelease HistoryDetailsSummary

Released

Journal Article

Response to Comment on “Following molecular mobility during chemical reactions: no evidence for active propulsion” and “Molecular diffusivity of click reaction components: the diffusion enhancement question”

MPS-Authors

/persons/resource/persons75462

Fischer, Peer
Max Planck Institute for Medical Research, Max Planck Society;

External Resource

https://pubs.acs.org/doi/full/10.1021/jacs.2c02830
(Any fulltext)

https://pubs.acs.org/doi/pdf/10.1021/jacs.2c02830
(Any fulltext)

Fulltext (restricted access)

There are currently no full texts shared for your IP range.

Fulltext (public)

There are no public fulltexts stored in PuRe

Supplementary Material (public)

There is no public supplementary material available

Citation

Fillbrook, L. L., Günther, J.-P., Majer, G., O’Leary, D. J., Price, W. S., Ryswyk, H. V., et al. (2022). Response to Comment on “Following molecular mobility during chemical reactions: no evidence for active propulsion” and “Molecular diffusivity of click reaction components: the diffusion enhancement question”. Journal of the American Chemical Society, 144, 13436-13440. doi:10.1021/jacs.2c02830.

Cite as: https://hdl.handle.net/21.11116/0000-000C-A42E-8

Abstract

In their Comment (DOI: 10.1021/jacs.2c02965) on two related publications by our groups (J. Am. Chem. Soc.2021, 143, 20884–20890; DOI: 10.1021/jacs.1c09455) and another (J. Am. Chem. Soc.2022, 144, 1380–1388; DOI: 10.1021/jacs.1c11754), Huang and Granick discuss the diffusion NMR measurements of molecules during a copper-catalyzed azide–alkyne cycloaddition (CuAAC) “click” reaction. Here we respond to these comments and maintain that no diffusion enhancement was observed for any species during the reaction. We show that the relaxation agent does not interfere with the CuAAC reaction kinetics nor the diffusion of the molecules involved. Similarly, the gradient pulse length and diffusion time do not affect the diffusion coefficients. Peak overlap was completely removed in our study with the use of hydrazine as the reducing agent. The steady-state assumption does not hold for these diffusion measurements that take several minutes, which is the reason monotonic gradient orders are not suitable. Finally, we discuss the other reactions where similar changes in diffusion have been claimed. Our conclusions are fully supported by the results represented in our original JACS Article and the corresponding Supporting Information.